Effects of mixing on evolution of hydrocarbon ratios in the troposphere

Nonmethane hydrocarbon (NMHC) concentration ratios provide useful indicators of tropospheric oxidation and transport processes. However, the influences of both photochemical and mixing processes are inextricably linked in the evolution of these ratios. We present a model for investigating these influences by combining the transport treatment of the Lagrangian particle dispersion model FLEXPART with an ultrasimple (i.e., constant OH concentration) chemical treatment. Required model input includes NMHC emission ratios, but not ad hoc assumed background NMHC concentrations. The model results give NMHC relationships that can be directly compared, in a statistical manner, with measurements. The measured concentration ratios of the longest-lived alkanes show strong deviations from purely kinetic behavior, which the model nicely reproduces. In contrast, some measured aromatic ratio relationships show even stronger deviations that are not well reproduced by the model for reasons that are not understood. The model-measurement comparisons indicate that the interaction of mixing and photochemical processing prevent a simple interpretation of "photochemical age," but that the average age of any particular NMHC can be well defined and can be approximated by a properly chosen and interpreted NMHC ratio. In summary, the relationships of NMHC concentration ratios not only yield useful measures of photochemical processing in the troposphere, but also provide useful test of the treatment of mixing and chemical processing in chemical transport models. Copyright 2007 by the American Geophysical Union

Establishing Lagrangian connections between observations within air masses crossing the Atlantic during the International Consortium for Atmospheric Research on Transport and Transformation experiment

The ITCT-Lagrangian-2K4 (Intercontinental Transport and Chemical Transformation) experiment was conceived with an aim to quantify the effects of photochemistry and mixing on the transformation of air masses in the free troposphere away from emissions. To this end, attempts were made to intercept and sample air masses several times during their journey across the North Atlantic using four aircraft based in New Hampshire (USA), Faial (Azores) and Creil (France). This article begins by describing forecasts from two Lagrangian models that were used to direct the aircraft into target air masses. A novel technique then identifies Lagrangian matches between flight segments. Two independent searches are conducted: for Lagrangian model matches and for pairs of whole air samples with matching hydrocarbon fingerprints. The information is filtered further by searching for matching hydrocarbon samples that are linked by matching trajectories. The quality of these "coincident matches'' is assessed using temperature, humidity and tracer observations. The technique pulls out five clear Lagrangian cases covering a variety of situations and these are examined in detail. The matching trajectories and hydrocarbon fingerprints are shown, and the downwind minus upwind differences in tracers are discussed

Climatological aspects of the extreme European rainfall of August 2002 and a trajectory method for estimating the associated evaporative source regions

International audienceDuring the first half of August 2002, a sequence of extreme precipitation episodes affected many regions of central and southern Europe, culminating in one of the most severe flooding events ever experienced along sections of the river Elbe and its tributaries. In this paper, the synoptic meteorological situation during the primary flooding event, 11-13 August 2002, and its recent background is illustrated and discussed. Then, backward trajectory modelling of water vapour transport is employed to determine the sources and transport pathways of the moisture which rained out during the event. The Lagrangian trajectory model FLEXTRA is used together with high resolution operational meteorological analyses from the ECMWF to track a very large number of trajectories, initialized in a dense three-dimensional grid array over the extreme rainfall region. Specific humidity changes along each trajectory are mapped out to yield source-receptor relationships between evaporation and subsequent precipitation for the event. Regions of significant surface evaporation of moisture which later rained out were determined to be parts of the Aegean and Ligurian Seas during the initial stages of the event, while strong evaporation from eastern European land surfaces and from the Black Sea became dominant later on. The method also provides precipitation estimates based solely on specific humidity changes along Lagrangian airmass trajectories, which can be compared to ECMWF model forecast precipitation estimates

The North Atlantic Oscillation controls air pollution transport to the Arctic

This paper studies the interannual variability of pollution pathways from northern hemisphere (NH) continents into the Arctic. Using a 15-year model simulation of the dispersion of passive tracers representative of anthropogenic emissions from NH continents, we show that the North Atlantic Oscillation (NAO) exerts a strong control on the pollution transport into the Arctic, particularly in winter and spring. For tracer lifetimes of 5 (30) days, surface concentrations in the Arctic winter are enhanced by about 70% (30%) during high phases of the NAO (in the following referred to as NAO⁺) compared to its low phases (NAO^-). This is mainly due to great differences in the pathways of European pollution during NAO⁺ and NAO^- phases, respectively, but reinforced by North American pollution, which is also enhanced in the Arctic during NAO⁺phases. In contrast, Asian pollution in the Arctic does not significantly depend on the NAO phase. The model results are confirmed using remotely-sensed NO₂ vertical atmospheric columns obtained from seven years of satellite measurements, which show enhanced northward NO₂ transport and reduced NO₂ outflow into the North Atlantic from Central Europe during NAO⁺ phases. Surface measurements of carbon monoxide (CO) and black carbon at high-latitude stations further corroborate the overall picture of enhanced Arctic pollution levels during NAO⁺ phase

Forecast, observation and modelling of a deep stratospheric intrusion event over Europe

A wide range of measurements was carried out in central and southeastern Europe within the framework of the EU-project STACCATO (Influence of Stratosphere-Troposphere Exchange in a Changing Climate on Atmospheric Transport and Oxidation Capacity) with the principle goal to create a comprehensive data set on stratospheric air intrusions into the troposphere along a rather frequently observed pathway over central Europe from the North Sea to the Mediterranean Sea. The measurements were based on predictions by suitable quasi-operational trajectory calculations using ECMWF forecast data. A predicted deep Stratosphere to Troposphere Transport (STT) event, encountered during the STACCATO period on 20-21 June 2001, could be followed by the measurements network almost from its inception. Observations provide evidence that the intrusion affected large parts of central and southeastern Europe. Especially, the ozone lidar observations on 20-21 June 2001 at Garmisch-Partenkirchen, Germany captured the evolution of two marked tongues of high ozone with the first one reaching almost a height of 2 km, thus providing an excellent data set for model intercomparisons and validation. In addition, for the first time to our knowledge concurrent measurements of the cosmogenic radionuclides <sup>10</sup>Be and <sup>7</sup>Be and their ratio <sup>10</sup>Be/<sup>7</sup>Be are presented together as stratospheric tracers in a case study of a stratospheric intrusion. The ozone tracer columns calculated with the FLEXPART model were found to be in good agreement with water vapour satellite images, capturing the evolution of the observed dry streamers of stratospheric origin. Furthermore, the time-height cross section of ozone tracer simulated with FLEXPART over Garmisch-Partenkirchen captures with many details the evolution of the two observed high-ozone filaments measured with the IFU lidar, thus demonstrating the considerable progress in model simulations. Finally, the modelled ozone (operationally available since October 1999) from the ECMWF (European Centre for Medium-Range Weather Forecasts) atmospheric model is shown to be in very good agreement with the observations during this case study, which provides the first successful validation of a chemical tracer that is used operationally in a weather forecast model. This suggests that coupling chemistry and weather forecast models may significantly improve both weather and chemical forecasts in the future

Export of Asian pollution during two cold front episodes of the TRACE-P experiment

Two cold front episodes were sampled during the two flights out of Yokota, Japan, during the Transport and Chemical Evolution Over the Pacific (TRACE-P) experiment during March 2001. The data from these two flights are examined using a mesoscale three-dimensional model. We show how these cyclonic systems have impacted the export of pollution out of the Asian continent. We contrast the relative role of convection and ascent in the warm conveyor belts associated with the cyclone during these two episodes. Although the necessary meteorological conditions for an efficient export of pollution are met during flight 13 (i.e., the occurrences of the warm conveyor belt near the source regions), no significant pollution is simulated in the mid-Pacific in the lower and middle troposphere. The efficient ventilation of the WCB by convection near the coast, the advection by the anticyclonical flow above 700 hPa, and the downward motion associated with the Pacific high in the remote ocean significantly prevent any long-range transport of undiluted pollution in the WCB. During flight 15 the conveyor belts have already moved to the remote ocean. The polluted plume is split by the rising air in the warm conveyor belt which transports CO-poor air northward and by the oceanic convection which transports clean air masses upward. These mechanisms lead to the dilution of Asian pollution in WCB en route to North America and add to the episodic nature of the Asian outflow by fragmenting the pollution plume

Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2

International audienceThe Lagrangian particle dispersion model FLEXPART was originally (about 8 years ago) designed for calculating the long-range and mesoscale dispersion of air pollutants from point sources, such as after an accident in a nuclear power plant. In the meantime FLEXPART has evolved into a comprehensive tool for atmospheric transport modeling and analysis. Its application fields were extended from air pollution studies to other topics where atmospheric transport plays a role (e.g., exchange between the stratosphere and troposphere, or the global water cycle). It has evolved into a true community model that is now being used by at least 25 groups from 14 different countries and is seeing both operational and research applications. A user manual has been kept actual over the years and was distributed over an internet page along with the model's source code. In this note we provide a citeable technical description of FLEXPART's latest version (6.2)

Quantifying wet scavenging processes in aircraft observations of nitric acid and cloud condensation nuclei

Wet scavenging is an important sink term for many atmospheric constituents. However, production of precipitation in clouds is poorly understood, and pollutant removal through wet scavenging is difficult to separate from removal through dry scavenging, atmospheric mixing, or chemical transformations. Here we use airborne data from the International Consortium for Atmospheric Research on Transport and Transformation project to show that measured ratios of soluble and insoluble trace gases provide a useful indicator for quantifying wet scavenging. Specifically, nitric acid (HNO3), produced as a by-product of combustion, is highly soluble and removed efficiently from clouds by rain. Regional carbon monoxide (CO), which is also an indicator of anthropogenic activity, is insoluble and has a lifetime against oxidation of about a month. We find that relative concentrations of HNO3 to regional CO observed in clear air are negatively correlated with precipitation production rates in nearby cloudy air (r2 = 0.85). Also, we show that relative concentrations of HNO3 and CO can be used to quantify cloud condensation nucleus (CCN) scavenging by precipitating clouds. This is because CCN and HNO3 molecules are both fully soluble in cloud water and hence can be treated as analogous species insofar as wet scavenging is concerned. While approximate, the practical advantage of this approach to scavenging studies is that it requires only measurement in clear air and no a priori knowledge of the cloud or aerosol properties involved

Sampling of an STT event over the Eastern Mediterranean region by lidar and electrochemical sonde

International audienceA two-wavelength ultraviolet (289?316nm) ozone Differential Absorption Lidar (DIAL) system is used to perform ozone measurements in the free troposphere in the Eastern Mediterranean (Northern Greece). The ozone DIAL profiles obtained during a Stratosphere-to-Troposphere Transport (STT) event are compared to that acquired by an electrochemical ozonesonde, in the altitude range between 2 and 10 km. The measurement accuracy of these two instruments is also discussed. The mean difference between the ozone profiles obtained by the two techniques is of the order of 1.11 ppbv (1.86%), while the corresponding standard deviation is 4.69 ppbv (8.16%). A case study of an STT event which occurred on 29 November 2000 is presented and analyzed, using ozone lidar, satellite and meteorological data, as well as air mass back-trajectory analysis. During this STT event ozone mixing ratios of 55?65 ppbv were observed between 5 and 7 km height above sea level (a.s.l.). Stratospheric air was mixed with tropospheric air masses, leading to potential vorticity (PV) losses due to diabatic processes. The ozone DIAL system can be used for following STT events and small-scale mixing phenomena in the free troposphere, and for providing sequences of vertical ozone profiles in the free troposphere. Keywords. Atmospheric composition and structure (Evolution of the atmosphere; Instruments and techniques) ? Meteorology and atmospheric dynamics (Middle atmosphere dynamics; Turbulence